Abstract
Owing to the different reaction properties and deactivation mechanisms caused by the structural discrepancy of monolithic catalysts, abundant scientific results of powder or granular NH3-SCR catalysts have still not sufficiently robustly applied in recent years. Furthermore, minimal research has been focused on monolithic catalysts. As a result, this work prepared monolithic Mn-Fe-Ce/Al2O3 catalysts by active component impregnation (ACI-Mn-Fe-Ce/Al2O3) and precursor impregnation methods (PI-Mn-Fe-Ce/Al2O3) and investigates the long-term SO2 and H2O resistance of the catalysts. Compared with the PI-Mn-Fe-Ce/Al2O3 catalyst, the monolithic ACI-Mn-Fe-Ce/Al2O3 catalyst showed better performance. The catalytic activity follows a bell-shaped curve with an optimal performance at a drug loading of 5 %. The ACI-Mn-Fe-Ce/Al2O3 catalyst exhibits long-term resistance to SO2 and H2O and can still convert more than 70 % NOx after 168 h of SO2 and H2O resistance test. Characterization of the ACI-Mn-Fe-Ce/Al2O3 catalysts before and after the reaction showed that the reducibility decreased after the reaction, and more Mn4+ was transformed into Mn2+ to weaken the catalytic activity. However, more Fe2+ and Ce3+ were generated during the reaction, increasing the number of oxygen vacancies, oxygen defects, and hydroxyl-like groups, all of which would contribute to a certain extent to counteract the passivation effect of SO2 on the catalysts. In situ DRIFTs analysis shows that the formation of surface sulfates has a minimal effect on the adsorption of NO, but it does affect the adsorption of coordinated NH3 on Lewis acid sites. This work elucidates the deactivation details of Mn-Fe-Ce/Al2O3 catalysts from the perspective of physicochemical properties, which provides a reference for the development of better low-temperature SO2-resistance catalysts for industrial applications.
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